Lithium Loss, Resistance Growth, Electrode Expansion, Gas Evolution, and Li Plating: Analyzing Performance and Failure of Commercial Large-Format NMC-Gr Lithium-Ion Pouch Cells

Gasper, Paul; Sunderlin, Nathaniel; Dunlap, Nathan; Walker, Patrick; Finegan, Donal P.; Smith, Kandler; Thakkar, Foram

doi:10.1016/j.jpowsour.2024.234494

Lithium Loss, Resistance Growth, Electrode Expansion, Gas Evolution, and Li Plating: Analyzing Performance and Failure of Commercial Large-Format NMC-Gr Lithium-Ion Pouch Cells

Journal Article · Sat Apr 06 04:00:00 EDT 2024 · Journal of Power Sources

DOI:https://doi.org/10.1016/j.jpowsour.2024.234494· OSTI ID:2342003

; Sunderlin, Nathaniel; Dunlap, Nathan; Walker, Patrick; ; ; Thakkar, Foram

Analysis of the performance evolution and failure mechanisms of commercial Li-ion batteries is crucial for improving testing methods, accurately modeling battery performance, and ensuring safe battery operation. Here, we present the results of a 2-year aging study conducted on commercial large-format LiNiMnCoO2-graphite pouch cells. Loss of lithium inventory (LLI) and loss of positive electrode active material (LAMPE) are shown to dominate capacity fade, as quantified by differential voltage-capacity analysis; only a small amount of LAMPE was measured in extracted electrode material, indicating that LAMPE in full cells was due to electrode dry-out. Resistance evolution, observed by direct current pulses and electrochemical impedance spectroscopy analyzed using the distribution of relaxation times, shows complex trends. Particle cracking and electrode expansion is theorized to cause most changes to resistance. Post-mortem measurements reveal a 10% increase in electrode stack thickness and substantial gas generation, with lithium plating observed in extreme cycling conditions, causing large resistance increases. Circumstantial evidence for self-discharge via redox shuttle, which decomposes the electrolyte, is shown. Overall, electrolyte stability was determined to be the limiting factor for cell lifetime. The impacts of many degradation mechanisms on diagnostic signals substantially overlap, making it challenging to monitor cell health and safety.

Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: Shell International Exploration & Production Inc.

DOE Contract Number:: AC36-08GO28308

OSTI ID:: 2342003

Report Number(s):: NREL/JA-5700-89744; MainId:90523; UUID:b82f86e5-b664-4049-bb61-1ed1e37221c4; MainAdminId:72487

Journal Information:: Journal of Power Sources, Journal Name: Journal of Power Sources Vol. 604

Country of Publication:: United States

Language:: English

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